Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries
Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries
复制标题
DOI：
10.1038/s41467-024-47521-z
复制
发表时间：
2024-04
影响因子：
16.6
通讯作者：
Jyotshna Pokharel;A. Cresce;Bharat Pant;Moon Young Yang;Ashim Gurung;Wei He;Abiral Baniya;B. Lamsal;Zhongjiu Yang;Stephen Gent;Xiaojun Xian;Ye Cao;William A. Goddard;Kang Xu;Yue Zhou
中科院分区：
文献类型：
--
作者：
Jyotshna Pokharel;A. Cresce;Bharat Pant;Moon Young Yang;Ashim Gurung;Wei He;Abiral Baniya;B. Lamsal;Zhongjiu Yang;Stephen Gent;Xiaojun Xian;Ye Cao;William A. Goddard;Kang Xu;Yue Zhou
在锂金属电极上构建人工固体电解质中间相（SEI）是解决锂金属电池发展中危险的锂形态（枝晶和死Li0）的猖獗生长和低库仑效率问题的一种有前途的方法，但SEI中的Li+传输行为如何与机械性能相结合仍然未知。我们在此展示了一种简便且可扩展的溶液处理方法，可形成富含 Li3N 的 SEI，其具有纯相晶体结构，可最大限度地减少 Li+ 穿过 SEI 的扩散能垒。与传统实践获得的多晶Li3N SEI相比，纯相/单晶富Li3N SEI构成了高机械强度和低Li+扩散势垒的界面。我们通过相场模拟与实验相结合，阐明了Li+迁移数、扩散行为、浓度梯度和锂金属电极稳定性之间的相关性。我们证明了用这种富含 Li3N SEI 构建的对称电池和全锂金属电池的可逆性和充电/放电循环行为得到了改善。这些研究可能为稳定和高性能锂金属电池的理想人工SEI的设计和工程提供新的见解。
Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrodes is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0) and low Coulombic efficiency that plague development of lithium metal batteries, but how Li+transport behavior in the SEI is coupled with mechanical properties remains unknown. We demonstrate here a facile and scalable solution-processed approach to form a Li3N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+across the SEI. Compared with a polycrystalline Li3N SEI obtained from conventional practice, the phase-pure/single crystalline Li3N-rich SEI constitutes an interphase of high mechanical strength and low Li+diffusion barrier. We elucidate the correlation among Li+transference number, diffusion behavior, concentration gradient, and the stability of the lithium metal electrode by integrating phase field simulations with experiments. We demonstrate improved reversibility and charge/discharge cycling behaviors for both symmetric cells and full lithium-metal batteries constructed with this Li3N-rich SEI. These studies may cast new insight into the design and engineering of an ideal artificial SEI for stable and high-performance lithium metal batteries.